As primary air pollutants, nitrogen oxides (NO x ) result in a series of environmental issues, such as photochemical smog, acid rain, ozone depletion, and fine particle pollution, which threaten the health of all human beings. Selective catalytic reduction with NH 3 (NH 3 -SCR) is the most powerful technique for the abatement of NO x . The development of NH 3 -SCR catalysts is the key to the normal operation of NO x removal systems. The currently used V 2 O 5 -WO 3 (MoO 3 )/TiO 2 catalysts are widely applicable for medium-/high-temperature conditions but are not suitable for NH 3 -SCR operated at low temperatures. The development of high-efficiency low-temperature SCR catalysts is the central issue at present. The rational design of efficient NH 3 -SCR catalysts requires an atomic-level understanding of their mode of operation, including the identification and characterization of the active sites, reaction paths, and rate-determining steps of NH 3 -SCR. Herein, we summarize the recent advances in catalysts for low-temperature NH 3 -SCR. The active sites, intermediates, and reaction pathways of oxide catalysts and molecular sieve catalysts mainly studied by researchers will be reviewed, with a particular focus on an atomic-level understanding of the mechanism. We provide an atomic-level understanding of the current general NH 3 -SCR catalytic mechanism and further combine the atomic-level understanding of the mechanism to provide design guidelines for low-temperature SCR catalysts. We hope that our account will trigger research activities and discussions in NH 3 -SCR catalysis and bridge the material gap between idealized and real catalytic systems.